Observation of the Brownian motion of a small probe interacting with its environment provides one of the main strategies for characterizing soft matter. Essentially, two counteracting forces govern the motion of the Brownian particle. First, the particle is driven by rapid collisions with the surrounding solvent molecules, referred to as thermal noise. Second, the friction between the particle and the viscous solvent damps its motion. Conventionally, the thermal force is assumed to be random and characterized by a Gaussian white noise spectrum. The friction is assumed to be given by the Stokes drag, suggesting that motion is overdamped at long times in particle tracking experiments, when inertia becomes negligible. However, as the particle receives momentum from the fluctuating fluid molecules, it also displaces the fluid in its immediate vicinity. The entrained fluid acts back on the particle and gives rise to long-range correlations. This hydrodynamic 'memory' translates to thermal forces, which have a coloured, that is, non-white, noise spectrum. One hundred years after Perrin's pioneering experiments on Brownian motion, direct experimental observation of this colour is still elusive. Here we measure the spectrum of thermal noise by confining the Brownian fluctuations of a microsphere in a strong optical trap. We show that hydrodynamic correlations result in a resonant peak in the power spectral density of the sphere's positional fluctuations, in strong contrast to overdamped systems. Furthermore, we demonstrate different strategies to achieve peak amplification. By analogy with microcantilever-based sensors, our results reveal that the particle-fluid-trap system can be considered a nanomechanical resonator in which the intrinsic hydrodynamic backflow enhances resonance. Therefore, instead of being treated as a disturbance, details in thermal noise could be exploited for the development of new types of sensor and particle-based assay in lab-on-a-chip applications.
The thermal position fluctuations of a single micron-sized sphere immersed in a fluid were recorded by optical trapping interferometry with nanometer spatial and microsecond temporal resolution. We find, in accord with the theory of Brownian motion including hydrodynamic memory effects, that the transition from ballistic to diffusive motion is delayed to significantly longer times than predicted by the standard Langevin equation. This delay is a consequence of the inertia of the fluid. On the shortest time scales investigated, the sphere's inertia has a small, but measurable, effect.
The equilibrium dynamics of a spherical particle immersed in a complex Maxwell fluid is analyzed in terms of velocity autocorrelation function (VACF), mean-square displacement (MSD), and power spectral density (PSD). We elucidate the role of hydrodynamic memory and its interplay with medium viscoelasticity for a free and a harmonically confined particle. The elastic response at high frequencies introduces oscillations in the VACF, which are found to be strongly damped by the coupling to the fluid. We show that in all Maxwell fluids hydrodynamic memory eventually leads to a power-law decay in the VACF as is already known for Newtonian fluids. The MSD displays asymptotically an intermediate plateau reflecting the elastic restoring forces of the medium. In the frequency domain, the PSD exhibits at high frequencies a step due to the trapping, whereas the low-frequency decay reflects the viscoelastic relaxation. Our results suggest that high-frequency microrheology is well-suited to infer the elastic modulus, which is sensitive over a wide range of Maxwell times.
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